CN101242888A - Oxygen isotope concentration method - Google Patents
Oxygen isotope concentration method Download PDFInfo
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- CN101242888A CN101242888A CNA2006800297064A CN200680029706A CN101242888A CN 101242888 A CN101242888 A CN 101242888A CN A2006800297064 A CNA2006800297064 A CN A2006800297064A CN 200680029706 A CN200680029706 A CN 200680029706A CN 101242888 A CN101242888 A CN 101242888A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D59/00—Separation of different isotopes of the same chemical element
- B01D59/50—Separation involving two or more processes covered by different groups selected from groups B01D59/02, B01D59/10, B01D59/20, B01D59/22, B01D59/28, B01D59/34, B01D59/36, B01D59/38, B01D59/44
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D59/00—Separation of different isotopes of the same chemical element
- B01D59/02—Separation by phase transition
- B01D59/04—Separation by phase transition by distillation
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D59/00—Separation of different isotopes of the same chemical element
- B01D59/34—Separation by photochemical methods
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D59/00—Separation of different isotopes of the same chemical element
- B01D59/28—Separation by chemical exchange
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- Oxygen, Ozone, And Oxides In General (AREA)
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Abstract
The method for concentrating an oxygen isotope or isotopes of the present invention combines the step of concentrating 17 O and/or the step of depleting 18 O that utilizes photodissociation of ozone by a laser beam with an oxygen distillation step that concentrates the oxygen isotope. At this time, it is preferable to carry out a step of isotope scrambling in addition to the above. When both a step of concentrating 17 O and a step of depleting 18 O are carried out, whichever thereof may be done first prior to the other. Also these steps may be placed either before or after the oxygen distillation step. Moreover, at least one of said oxygen distillation step, the concentrating 17 O step, the depleting 18 O step and the isotope scrambling step is preferably carried out twice or more. According to the invention, low abundance ratio oxygen stable isotope 17 and 18 can be concentrated into high concentration effectually under technical scale.
Description
Technical field
The present invention relates to the method for concentration of oxygen isotope.Specifically, the laser isotope separation and the separated that relate to utilizing the ozone photolysis of being undertaken by laser make up, thus effectively that abundance ratio is very little oxygen stable isotope
17O is condensed into the method for high concentration and simultaneously will
17O and
18O is condensed into the method for high concentration.
The application quotes its content based on the Japanese Patent Application 2005-236499 number opinion priority of on August 17th, 2005 in Japanese publication at this.
Background technology
Oxygen stable isotope
16O,
17O and
18Among the O, owing to have only
17O has nuclear spin, therefore uses
17The compound of O mark is used for researchs such as the structural analysis undertaken by nuclear magnetic resonance, and is used as tracer in fields such as chemistry and medical science.In addition, the diagnostic agent of the positive electron laminagraphy diagnosis of using as the inspection that is used for tumour etc. (PET)
18The raw material of FDG (the PET contrast preparation that obtains with the fluorine 18 labelled with radioisotope FDGs of positive electron release nucleic), the utilization of expectation in medical field.
That is,
17O and
18O is an isotope useful on the industry, still, because natural abundance ratio is very little, need concentrate from the compound that contains oxygen atom when using it
17O and/or
18O.
Known is existing
17The method for concentration of O for example has following method.
That is, known have: with water as raw material, by it is distilled with
17O is concentrated into 25atom%, further, is concentrated into the method (with reference to non-patent literature 1) of 90atom% by thermal diffusion; Nitric oxide (NO) is as raw material, concentrated by it is distilled
17O further, is condensed into the method (non-patent literature 4) of high concentration (for example 40atom%) by thermal diffusion; With oxygen as raw material, by it is distilled with
17O is concentrated into the method (with reference to patent documentation 1) of 10atom%; Make its method of predissociationing and concentrating (with reference to non-patent literature 2, patent documentation 5 and patent documentation 6) by PARA FORMALDEHYDE PRILLS(91,95) irradiation Ne ion laser; Method (with reference to non-patent literature 3) to ozone irradiation visible light and ultraviolet light; And the use semiconductor laser, specific to containing
17The ozone of O carries out photodissociation, concentrates in oxygen
17The method of O (with reference to patent documentation 2,3 and 4) etc.
Patent documentation 1: international open WO00/27509 communique
Patent documentation 2: TOHKEMY 2004-261776 communique
Patent documentation 3: TOHKEMY 2005-040668 communique
Patent documentation 4: international open WO2004/078325 communique
Patent documentation 5: No. 4029559 specification of United States Patent (USP)
Patent documentation 6: No. 4029558 specification of United States Patent (USP)
Non-patent literature 1:I.Dostrovsky; " The production of stable isotopes ofoxygen " Analytical Chemistry Symposium Series pp693-702 (1982)
Non-patent literature 2:Jack Marling: " isotope separation of oxygen-17; oxygen-18; carbon-13and deuterium by ion laser induced formaldehydephotopredissociation ", The Journal of Chemical Physics, vol.66, no.9, p.4200-4225 (1977)
Non-patent literature 3:J.Wen and Mark H.Thiemens: " Experimental and theoretical study of isotope effects on ozone decomposition ", J.GeophysicalResearch, vol.96, no.D6, p.10911-10921 (1991)
Non-patent literature 4:McInteer, B.B.; Potter, Robert M.: " Nitric oxid distillation plant for isotope separation ", Ind.Eng.Chem., Process Design Develop., 4 (1), pp35-42 (1965)
But, in the method for non-patent literature 1 record, if consider that yield then exists resulting
17Be limited to the problem of several atom% degree in the O practicality, in the method for non-patent literature 4 records, concentrate by this method for concentration
17O is as H
2O or O
2On market, sell, but exist it to concentrate the inadequate problem of amount.
In addition, in non-patent literature 2, patent documentation 5 and the patent documentation 6 method of record also exist enrichment factor insufficient, also do not establish the problem of the technology of carrying out under the commercial scale.
Further, in the method for non-patent literature 3 records, can in remaining ozone, concentrate
17O and
18O confirms the isotope effect that ozone decomposes, but is not the enrichment factor that can be used in the isotopic separation degree.In addition, do not establish the technology of carrying out under the commercial scale yet.
On the other hand, the method for record is the method that is expected in industrial realization in the patent documentation 2,3 and 4, but because there is overlapped part in the laser absorption wave-length coverage of each ozone isotopic molecule, is particularly containing
17When the abundance ratio of the ozone molecule of O is little, though want by laser optionally only the disassociation contain
17The ozone molecule of O also can dissociate simultaneously
16O
3Etc. the bigger isotopic molecule of abundance ratio.Therefore, existence is difficult to obtain effectively high concentration
17The problem of O.
Below, from being elaborated with the method for related angle of the present invention to patent documentation 1 record.
Contain
16O,
17O and
18Its vapour pressure of the isotopic molecule of O (boiling point) is all very approaching, contains
17The isotopic molecule of O is to contain
16The isotopic molecule of O and containing
18(vapour pressure or boiling point exist the inter-level of the isotopic molecule of O
16O and
18Between the O),
17The natural abundance ratio of O is about 370atomppm, less than
18The 2000atomppm of O.Therefore, undertaken by distillation as patent documentation 1 is disclosed
17In the method for concentration of O, exist to be difficult to obtain effectively high concentration (for example more than the 5atom%)
17The problem of O.To this, carry out specific description by following example.
Figure 22 is used for the compound that contains oxygen atom (H for example
2O, NO, O
2Deng) distill, improve
17O or
18The skeleton diagram of the destilling tower 1 of O isotopes concentration.In fact, in most cases because the height (theoretical cam curve) of the destilling tower that requires is very high, the destilling tower that therefore actual device uses a plurality of destilling towers to be in series usually carries out a series of distillation procedure, but simplify at this, represent with a destilling tower.
Near cat head pars intermedia is supplied with oxygen to destilling tower 1 isotopic abundance ratio is raw material F (for example, the H of natural abundance ratio as shown in table 1
2O, NO, O
2Deng), collect concentrated from tower bottom
17O or
18The product P 1 of O.In addition, also exist, compare the tower pars intermedia of tower bottom side with the supply position of raw material F and collect concentrated with product P 1
17O or
18The situation of the other products P2 of O.Compare with raw material F and to have reduced
17O or
18The waste gas W of O discharges from top of tower.
[table 1]
Isotope | Atomic weight | Abundance ratio |
16O 17O 18O | 16 17 18 | 0.99759 0.00037 0.00204 |
Tower bottom at this destilling tower 1 concentrates
17O, when collecting product P 1 at the bottom of the tower, the isotopes concentration in the destilling tower distributes roughly as shown in figure 23.The longitudinal axis of Figure 23 is represented the concentration (atom%) of each oxygen isotope, and transverse axis is represented the height of destilling tower, among this figure afterwards too.Product P 1
17Though the enrichment of O according to height (theoretical cam curve) difference of destilling tower, is generally the scope of 0.2~5atom%.In the example of Figure 23, product P 1
17The O enrichment is about 1atom%.
On the other hand, in order to obtain highly enriched degree (for example more than the 5atom%)
17O, the destilling tower of needs higher (theoretical cam curve is many).At this moment, as shown in figure 24, because than
17The composition that the O boiling point is high
18O is condensed into high concentration at tower bottom, tower bottom
17The O enrichment reduces,
17The concentration of O is formed on the distribution that the pars intermedia of tower has maximum.That is, destilling tower 1 inside can be divided into from raw material F supply with the position to
17Till the O concentrate P2 assembling position
17The interval A that the O enrichment increases, and from
17O concentrate P2 assembling position arrives
18Till the O concentrate P1 assembling position
18The interval B that the O enrichment increases is in order to make
17O concentrate P2 assembling position
17O enrichment bigger (for example more than the 5atom%) must increase the height of interval A and interval B, and this method for concentration can not be realized industrial as far as possible.
Further, distil process needs a large amount of liquid column reserves in installing on its principle, thus exist for natural abundance than being at most the 370ppm degree
17O is condensed into high concentration (for example more than the 5atom%), and the starting time of device needs above problem for a long time of several years.
For the above reasons, we can say only will by distillation
17O is condensed into high concentration (for example more than the 8atom%) and realizes in industrial being difficult to.
Summary of the invention
Therefore, the object of the present invention is to provide a kind of
17The O method for concentration, can be under commercial scale effectively and high concentration concentrate the very little oxygen stable isotope of abundance ratio
17O.In addition, provide with
17When being condensed into high concentration, O also can concentrate
18The method of O.
In order to address the above problem, a first aspect of the present invention is a kind of method for concentration of oxygen isotope, comprises the distillation process of the isotopic oxygen of concentrate oxygen and ozone is carried out photodissociation and the concentrate oxygen isotope
17The operation of O.
In the method for concentration of oxygen isotope of the present invention, preferably include the operation of carrying out isotope conversion (isotopescrambling).
In addition, in the method for concentration of oxygen isotope of the present invention, preferably include ozone is carried out photodissociation and reduces oxygen isotope
18The operation of O.
In addition, in the method for concentration of oxygen isotope of the present invention, preferably to the distillation process of the isotopic oxygen of concentrate oxygen, ozone is carried out photodissociation and the concentrate oxygen isotope
17The operation of O, ozone is carried out photodissociation and reduces oxygen isotope
18The operation of O and at least a operation of carrying out in the operation of isotope conversion are carried out more than twice.
In addition, in the method for concentration of oxygen isotope of the present invention, oxygen isotope can reduced
18Carry out the concentrate oxygen isotope after the operation of O
17The operation of O also can carried out the concentrate oxygen isotope
17Reduce oxygen isotope after the operation of O
18The operation of O.
A second aspect of the present invention is a kind of manufacture method of heavy oxygen water, to what obtain by method for concentrating oxygen isotope of the present invention
17The O concentrate oxygen and/or
18The O concentrate oxygen adds hydrogen, obtains oxygen isotope
17O and/or oxygen isotope
18O is condensed into the water of the above concentration of 1atom%.
By the method for concentration of oxygen isotope of the present invention, can obtain high concentration effectively
17O.In addition, when concentrating, owing to compared with prior art finish with the short starting time, can be with low-cost and under commercial scale, obtain high concentration
17O.At this moment, owing to can easily carry out from ozone carrying out to the conversion of oxygen or from the conversion of oxygen to ozone
17During O concentrated, can make up various steps, thereby can select to meet desirable
17The step of O concentration and output.In addition, concentrate high concentration from feed oxygen
17During O, concentrating
17The operation of O and minimizing
18In the operation of O, can separate, reclaim high concentration from feed oxygen
18O.Thus, obtain high concentration
17Also can obtain high concentration in the time of O
18O.
Further, use method for concentration by oxygen isotope of the present invention to obtain
17The O concentrate oxygen or
18The O concentrate oxygen can and obtain having concentrated under commercial scale with low cost
17O or
18The heavy oxygen water of O.
Description of drawings
Fig. 1 is the skeleton diagram of expression first embodiment of the invention.
The skeleton diagram of the separation by laser device that Fig. 2 uses among one routine the present invention for expression.
Fig. 3 forms the figure that distributes for oxygen isotope in the destilling tower in the expression first embodiment of the invention.
Fig. 4 is the skeleton diagram of expression second embodiment of the invention.
Fig. 5 forms the figure that distributes for oxygen isotope in the destilling tower in the expression second embodiment of the invention.
Fig. 6 is the skeleton diagram of expression third embodiment of the invention.
The skeleton diagram of the separation by laser device that Fig. 7 uses in the one routine third embodiment of the invention for expression.
The skeleton diagram of the separation by laser device that Fig. 8 uses in the one routine third embodiment of the invention for expression.
Fig. 9 forms the figure that distributes for oxygen isotope in the destilling tower in the expression third embodiment of the invention.
Figure 10 is the skeleton diagram of expression four embodiment of the invention.
Figure 11 forms the figure that distributes for oxygen isotope in the destilling tower in the expression four embodiment of the invention.
Figure 12 is the skeleton diagram of expression fifth embodiment of the invention.
Figure 13 forms the figure that distributes for oxygen isotope in the destilling tower in the expression fifth embodiment of the invention.
Figure 14 is the skeleton diagram of expression sixth embodiment of the invention.
Figure 15 forms the figure that distributes for oxygen isotope in the destilling tower in the expression sixth embodiment of the invention.
Figure 16 is the skeleton diagram of expression seventh embodiment of the invention.
Figure 17 forms the figure that distributes for oxygen isotope in the destilling tower in the expression seventh embodiment of the invention.
Figure 18 is the skeleton diagram of expression eighth embodiment of the invention.
Figure 19 forms the figure that distributes for oxygen isotope in the destilling tower in the expression eighth embodiment of the invention.
Figure 20 is the skeleton diagram of expression ninth embodiment of the invention.
Figure 21 forms the figure that distributes for oxygen isotope in the destilling tower in the expression ninth embodiment of the invention.
Figure 22 is the skeleton diagram that the existing oxygen isotope of expression one example concentrates the middle destilling tower that uses.
The figure that Figure 23 distributes for the isotopes concentration in the expression one routine destilling tower.
The figure that Figure 24 distributes for the isotopes concentration in the many destilling towers of expression one routine theoretical cam curve.
Symbol description
1,6 destilling tower
2 ozone separators (A type)
3 isotope converters (isotope scrambler)
4,5 ozone separators (Type B)
The specific embodiment
Below the present invention is described in detail.
The present invention is will by the technology of design
17O is condensed into the method for high concentration (for example more than the 5atom%), and described design utilizes to greatest extent uses distilling apparatus
17The O method for concentration
17O concentrated effect and use the laser isotope separator (being designated hereinafter simply as the separation by laser device) utilize the ozone photolysis
17The O method for concentration
17The O concentrated effect.
Specifically, this method is to concentrate by distillation at low concentration region (for example 370atomppm~0.2atom% degree)
17O, this low enrichment that will obtain by distillation again
17O further concentrates by separation by laser, thereby obtains high concentration (for example more than the 5atom%)
17O.
In addition, this method is removed effectively by the separation by laser device that is connected with this destilling tower and is being concentrated by distillation
17Become obstruction during O
18O promotes in this destilling tower
17O concentrates.In addition, this method obtains ultrahigh concentration with the combination of these methods, for example more than 70%
17O.
Among the present invention, use separation by laser device
17There are two kinds of methods in the O method for concentration.
That is containing in ozone gas,
16O,
17O and
18In the ozone molecule of O, will optionally decompose and contain
17The ozone molecule of O obtains
17The O concentrate oxygen separated from above-mentioned containing each isotopic ozone gas, thereby concentrated
17The method of O; And will optionally decompose and contain
18The ozone molecule of O obtains
18The O concentrate oxygen was removed from above-mentioned containing each isotopic ozone gas, thereby reduced
18The method of O.
Among the present invention, by concentrating to above-mentioned
17The operation of O and/or minimizing
18The operation of O makes up with the operation of distillation oxygen, can carry out effectively
17O concentrates.At this moment, by further adding the operation of carrying out the isotope conversion, can more effectively carry out
17O concentrates.
In addition, concentrate
17The operation of O and minimizing
18The operation of O both the time, the order of carrying out is not limited especially.In addition, these operations can be carried out arbitrarily in the front and back of the operation of distilling oxygen.
Further, by to the operation of distillation oxygen, concentrate
17The operation of O, minimizing
18The operation of O and at least a operation of carrying out in the operation of isotope conversion are carried out more than twice, can more effectively carry out
17O concentrates.
In addition, concentrate high concentration from feed oxygen
17During O, concentrating
17The operation of O and minimizing
18In the operation of O, separation from feed oxygen, recovery high concentration
18O.Thus, obtain high concentration
17Also can obtain high concentration in the time of O
18O (for example more than the 20atom%).
For what obtain by the present invention
17O concentrate oxygen (for example more than the 5atom%) or
18O concentrate oxygen (for example more than the 20atom%), according to conventional methods, for example, the hydrogen with adding after the argon diluent corresponding to this oxygen amount reacts under the temperature more than 80 ℃ in platinum catalyst, and can make oxygen isotope thus is that 1atom% is above
17The O condensed water or
18The O condensed water.
<the first embodiment 〉
The most basic embodiment of the present invention, promptly first embodiment skeleton diagram as shown in Figure 1.Present embodiment is used to have connected and is used to distill oxygen and the device of isotopic destilling tower 1 of separated oxygen and separation by laser device 2 is characterized in that,
17The low concentration region of O carries out the phase I by distillation
17O concentrates, and for example exists
17O reach 0.2atom% above after, carry out separation by laser as second stage
17O concentrates.Thus, can concentrate effectively
17O.
Raw material F is fit to use ultra-high purity oxygen.As ultra-high purity oxygen, for example preferably from tonnage oxygen, remove argon, hydrocarbon etc., significantly improve the ultra-high purity oxygen of the chemical purity of oxygen.In addition, as the oxygen destilling tower, the destilling tower that also can use a plurality of destilling towers to be connected in series to form substitutes destilling tower 1.On the other hand, for the filler in the destilling tower, any one of service regeulations filler and irregular filler can obtain identical effect.
For the filler in raw material, oxygen destilling tower and the destilling tower, also identical in other embodiments.
The structure of the separation by laser device 2 that uses in the present embodiment (A type) is identical with disclosed apparatus structure in the patent documentation 2 and 3 for example.One is for example shown in Figure 2.
That is, in destilling tower 1, carry out the phase I
17After O concentrates, with oxygen F
LISImport in the ozone generator 21 and generate ozone, with ozone-oxygen gas mixture of producing with diluent gas (Kr) with after reclaiming diluent gas and mixing, use ozone separator 22, separation ozone and oxygen from this mist.Oxygen that separates and oxygen F from destilling tower 1
LISMix, be used for the generation of ozone once more.On the other hand, the ozone that separates is sent in the separation by laser device 23 with diluent gas, the laser of irradiation specific wavelength will contain
17The ozone of O optionally is decomposed into oxygen.With concentrating of obtaining here
17The oxygen of O, undecomposed ozone and diluent gas are sent in the oxygen retracting device 24, are concentrated
17The oxygen P of O
LISRemaining undecomposed ozone and diluent gas are sent in the ozonolysis equipment 25, all ozone is decomposed into oxygen.The oxygen and the diluent gas that produce are sent in the diluent gas retracting device 26, separate
17O is reduced,
18The oxygen W that O is concentrated
LIS, the diluent gas of recovery adds in the ozone generator 21 in the mist of the ozone that generates and oxygen once more.
In addition, use the diluent gas of Kr in the present embodiment, but dilute ozone, also can be other gas so long as can not damage effect of the present invention as ozone.
And separation by laser device (LIS unit) is separated into the function that isotope concentrate oxygen and isotope reduce oxygen as long as have the photolysis of utilizing ozone with feed oxygen, does not then limit especially for the detailed step in the LIS unit.
The above is also identical in other embodiment.
Present embodiment is specific as follows.That is, will improve by distillation
17The oxygen D of O concentration
Bot(the F among Fig. 2
LIS) extract out from the tower bottom of destilling tower 1, being sent in the separation by laser device 2, selectivity decomposition as described above contains
17The ozone of O obtains thus
17Oxygen P (the P among Fig. 2 that O is concentrated
LIS).The waste gas W1 that produces during distillation is discarded from the top of tower of destilling tower 1, the waste gas W2 (W among Fig. 2 that produces during separation by laser
LIS) discarded from separation by laser device 2.But waste gas W2 is owing to compare further concentrated with raw material F
17O and
18Therefore O also can supply to other
17The O concentration step or
18In the O concentration step.The utilization again of this waste gas W2 also can similarly be carried out in following all embodiments.
The destilling tower that uses specification shown in the table 3 as destilling tower 1, use specification shown in the table 4 the separation by laser device as separation by laser device 2, use the ultra-high purity oxygen of forming shown in the table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in the table 5.Further, the isotopics distribution table of the oxygen in the destilling tower 1 is shown among Fig. 3.In addition, each isotopic purity (atom%) shown in the table 5 is to use the value of the amount that contains each isotopic oxygen (mol%) that obtains by simulation, and according to the value that the calculating formula shown in table 5 below is tried to achieve, this is also identical in other embodiment.In addition, the distillation calculation procedure write up that uses in this simulation is in the WO00/27509 communique.On the other hand, the composition of the ultrahigh concentration oxygen F of table 2 is tried to achieve by the natural abundance ratio of table 1.
[table 2] calculated by the natural abundance ratio of table 1
Isotope | Atomic weight | Abundance ratio |
16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 32 33 34 34 35 36 | 0.99519 0.00074 0.00407 1.37×10 -7 1.51×10 -6 4.16×10 -6 |
[table 3]
Destilling tower kind tower diameter packed height filler operating pressure reboiler heat exchange amount | Packed tower 0.120m 150m Φ 5mm Raschig ring (Raschig ring) 20kPa (G) 2.7kW |
[table 4]
LIS unit (A type) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 5.88E-06 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 4.12E-05 | 1.00 | - | - |
(3) | The ozone generator outlet | 3.92E-05 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 7.45E-05 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 3.53E-05 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS charging (O 3,Kr) | 3.92E-05 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 3.93E-05 | 0.01 | 0.10 | 0.90 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2 | 2.33E-07 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 3.91E-05 | - | 0.10 | 0.90 |
(10) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 4.10E-05 | 0.14 | - | 0.86 |
(11) | Kr reclaims outlet (Kr): the Kr internal circulating load | 3.53E-05 | - | - | 1.00 |
(12) | Kr reclaims outlet (O 2): LIS reduces O 2 | 5.65E-06 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 6.78E-04 3.08E-03 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser | 16O 16O 17O 90% 0.009 |
[table 5]
F | W1 | D bot | W2 | P | ||
Flow [mol/s] | 1.0e-3 | 9.94e-4 | 5.88e-6 | 5.65e-6 | 2.33e-7 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 9.95e-1 7.38e-4 4.07e-3 1.37e-7 1.51e-6 4.16e-6 | 9.98e-1 6.20e-4 1.17e-3 3.94e-8 2.47e-7 4.55e-7 | 4.84e-1 2.07e-2 4.94e-1 1.66e-5 2.15e-4 6.31e-4 | 5.48e-1 1.05e-2 3.74e-1 5.07e-5 3.59e-3 6.37e-2 | 5.93e-1 1.41e-1 2.13e-1 8.36e-3 2.53e-2 1.91e-2 |
Isotopic purity [atom%] | 16O 17O 18O | 9.98e-1 3.70e-4 2.04e-3 | 9.99e-1 3.10e-4 5.85e-4 | 7.42e-1 1.05e-2 2.48e-1 | 7.41e-1 7.12e-3 2.52e-1 | 7.70e-1 9.14e-2 1.38e-1 |
16The O isotopic purity=
16O
2+
16O
17O/2+
16O
18O/2
17The O isotopic purity=
17O
2+
16O
17O/2+
17O
18O/2
18The O isotopic purity=
18O
2+
16O
18O/2+
17O
18O/2
<the second embodiment 〉
In the present embodiment, be connected with isotope converter 3 on the destilling tower 1 in the first embodiment.Its skeleton diagram as shown in Figure 4.
In addition, isotope converter 3 is when having multiple isotopic molecule, promotes each molecule optionally to change the phenomenon of the pairing atom of its formation, promptly promote the device that isotope is changed, and its concrete function write up is in the WO00/27509 communique.
The link position of isotope converter 3 can be at any part of destilling tower.From destilling tower 1, extract portion gas out, the gas of extracting out is sent to carries out the isotope conversion in the isotope converter 3, return destilling tower.At this moment, preferably carry out from destilling tower 1 gas bleeding from position or tower bottom near tower bottom.In addition, the position that the gas after the isotope conversion is returned in the destilling tower 1 does not limit especially, can be near the position of gas bleeding or identical position yet.
That is, present embodiment is characterised in that, on the isotope concentrated effect basis in the first embodiment, further uses isotope converter 3 to promote in the destilling tower
17O and
18O concentrates, and can improve product P
17The O enrichment.
The destilling tower that uses specification shown in the table 3 as destilling tower 1, use specification shown in the table 6 the separation by laser device as separation by laser device 2, use the ultra-high purity oxygen of forming shown in the table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in table 7 and the table 8.Further, the isotopics distribution table of the oxygen in the destilling tower 1 is shown among Fig. 5.
And in this simulation, the gas in the employing destilling tower 1 is with 1.0 * 10
-3Mol/s extracts out from tower bottom, returns the condition of tower bottom after handling with isotope converter 3.
[table 6]
LIS unit (A type) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 6.19E-06 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 4.34E-05 | 1.00 | - | - |
(3) | The ozone generator outlet | 4.13E-05 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 7.85E-05 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 3.72E-05 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS charging (O 3,Kr) | 4.13E-05 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 4.14E-05 | 0.01 | 0.10 | 0.90 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2 | 2.78E-07 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 4.11E-05 | - | 0.10 | 0.90 |
(10) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 4.31E-05 | 0.14 | - | 0.86 |
(11) | Kr reclaims outlet (Kr): the Kr internal circulating load | 3.72E-05 | - | - | 1.00 |
(12) | Kr reclaims outlet (O 2): LIS reduces O 2 | 5.92E-06 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 7.14E-04 3.24E-03 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser | 16O 16O 17O 90% 0.011 |
[table 7]
F | W1 | S in | S out | ||
Flow [mol/s] | 1.0e-3 | 9.94e-4 | 1.0e-3 | 1.0e-3 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 9.95e-1 7.38e-4 4.07e-3 1.37e-7 1.51e-6 4.16e-6 | 9.98e-1 5.77e-4 1.02e-3 7.25e-8 2.26e-7 3.50e-7 | 5.48e-1 1.99e-2 3.65e-1 1.79e-4 6.56e-3 6.02e-2 | 5.48e-1 1.98e-2 3.65e-1 1.80e-4 6.60e-3 6.06e-2 |
Isotopic purity [atom%] | 16O 17O 18O | 9.98e-1 3.70e-4 2.04e-3 | 9.99e-1 2.89e-4 5.12e-4 | 7.40e-1 1.34e-2 2.46e-1 | 7.40e-1 1.34e-2 2.46e-1 |
[table 8]
D bot | W2 | P | ||
Flow [mol/s] | 6.19e-6 | 5.92e-6 | 2.78e-7 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 5.46e-1 1.99e-2 3.66e-1 1.79e-4 6.59e-3 6.07e-2 | 5.45e-1 1.36e-2 3.73e-1 8.44e-5 4.64e-3 6.37e-2 | 5.79e-1 1.57e-1 2.07e-1 1.07e-2 2.81e-2 1.85e-2 |
Isotopic purity [atom%] | 16O 17O 18O | 7.39e-1 1.34e-2 2.47e-1 | 7.38e-1 9.19e-3 2.52e-1 | 7.61e-1 1.03e-1 1.36e-1 |
<the three embodiment 〉
Present embodiment has been improved first embodiment, has realized
17The raising of the further concentrated and yield of O.Its skeleton diagram as shown in Figure 6.
Separation by laser device 4 (Type B) is for carrying out the device of separation by laser in two stages.It can be that the separation by laser device 2 (A type) that will use in 2 first embodiments is formed by connecting as shown in Figure 7, this device also can be brought into play same function, but for example the device of structure shown in Figure 8 is preferred because ozone generator or diluent gas retracting device are become one.
That is, in destilling tower 1, carry out the phase I
17After the concentrating of O, with oxygen F
LISImport in the ozone generator 41 and generate ozone, with ozone-oxygen gas mixture of producing with diluent gas (Kr) with after reclaiming diluent gas and mixing, use ozone separator 42, separation ozone and oxygen from this mist.Oxygen that separates and oxygen F from destilling tower 1
LISMix, be used to generate ozone once more.On the other hand, the ozone that separates is sent in the first separation by laser device 43 with diluent gas, the laser of irradiation specific wavelength will contain
17The ozone of O optionally is decomposed into oxygen.With containing of obtaining here
17The oxygen of O, undecomposed ozone and diluent gas are sent in the first oxygen retracting device 44, obtain
17O enriched gaseous oxygen P1
LISRemaining undecomposed ozone and diluent gas are sent in the second separation by laser device 45, and the laser of irradiation specific wavelength will contain
18The ozone of O optionally is decomposed into oxygen.With containing of obtaining here
18The oxygen of O, undecomposed ozone and diluent gas are sent in the second oxygen retracting device 46, obtain
18O enriched gaseous oxygen P2
LISRemaining undecomposed ozone and diluent gas are sent in the ozonolysis equipment 47, and all ozone is decomposed into oxygen.The oxygen and the diluent gas that produce are sent in the diluent gas retracting device 48, separate
17O and
18The oxygen W that O reduces
LIS, the diluent gas of recovery adds in the ozone generator 41 in the mist of the ozone that generates and oxygen once more.
In the first embodiment, the oxygen of collecting from the tower bottom of destilling tower 1 imports to separation by laser device 2, optionally decomposes and contains
17The ozone molecule of O
16O
16O
17O obtains having concentrated thus
17The oxygen P of O is in order to prevent in the destilling tower 1
18O concentrates and to be caused
17The O enrichment reduces, and is remaining
17O reduces oxygen and does not turn back in the destilling tower 1, and discarded as W2.This is owing to if will concentrate
18The W2 of O turns back in the destilling tower 1, then
18O further concentrates at the bottom of the tower of destilling tower 1, meanwhile reduces at the bottom of the tower of destilling tower 1
17The enrichment of O.
On the other hand, present embodiment in the following way: from reducing by the phase I separation by laser
17In the ozone of O, optionally decompose by the second stage separation by laser and contain
18The ozone molecule of O
16O
16O
18O removes concentrated thus
18The oxygen of O, its remaining oxygen R (W among Fig. 8
LIS) turn back to the destilling tower pars intermedia by air blast (diagram slightly) etc.Thus, can prevent in the destilling tower 1
18When concentrating, O promotes
17O concentrates, thereby can improve
17The O yield.
The destilling tower that uses specification shown in the table 3 as destilling tower 1, use specification shown in the table 10 the separation by laser device as separation by laser device 4, use the ultra-high purity oxygen of forming shown in the table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in the table 9.Concentrating among the P1 as can be known has
17Concentrating among O, the W2 has
18O.
Further, the isotopics distribution table of the oxygen in the destilling tower 1 is shown among Fig. 9.
[table 9]
F | W1 | D bot | R | W2 | P1 | ||
Flow [mol/s] | 1.00e-3 | 9.95e-4 | 1.29e-5 | 7.47e-6 | 4.86e-6 | 5.38e-7 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 9.95e-1 7.38e-4 4.07e-3 1.37e-7 1.51e-6 4.16e-6 | 9.98e-1 5.99e-4 1.10e-3 5.03e-8 2.36e-7 4.03e-7 | 5.15e-1 2.03e-2 4.32e-1 7.06e-5 2.86e-3 3.00e-2 | 5.82e-1 1.60e-2 3.45e-1 1.10e-4 4.75e-3 5.12e-2 | 4.95e-1 5.73e-3 4.11e-1 1.66e-5 2.38e-3 8.53e-2 | 5.87e-1 1.48e-1 2.10e-1 9.33e-3 2.65e-2 1.88e-2 |
Isotopic purity [atom%] | 16O 17O 18O | 9.98e-1 3.70e-4 2.04e-3 | 9.99e-1 3.00e-4 5.50e-4 | 7.41e-1 1.17e-2 2.47e-1 | 7.63e-1 1.05e-2 2.26e-1 | 7.04e-1 4.07e-3 2.92e-1 | 7.66e-1 9.66e-2 1.37e-1 |
[table 10]
LIS unit (Type B) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 1.29E-05 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 9.01E-05 | 1.00 | - | - |
(3) | The ozone generator outlet | 8.58E-05 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 1.63E-04 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 7.72E-05 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS phase I charging (O 3,Kr) | 8.58E-05 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 8.59E-05 | 0.01 | 0.10 | 0.90 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2-1 | 5.38E-07 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=LIS second stage charging (O 3,Kr) | 8.54E-05 | - | 0.10 | 0.90 |
(10) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 8.70E-05 | 0.06 | 0.06 | 0.89 |
(11) | O 2Knockout tower cat head=LIS concentrates O 2-2 | 4.86E-06 | 1.00 | - | - |
(12) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 8.22E-05 | - | 0.06 | 0.94 |
(13) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 8.47E-05 | 0.09 | - | 0.91 |
(14) | Kr reclaims outlet (Kr): the Kr internal circulating load | 7.72E-05 | - | - | 1.00 |
(15) | Kr reclaims outlet (O 2): LIS reduces O 2 | 7.47E-06 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 1.48E-03 6.74E-03 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (phase I) | 16O 16O 17O 90% 0.022 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (second stage) | 16O 16O 18O 90% 0.195 |
<the four embodiment 〉
The 3rd embodiment concentrates in the separation by laser of phase I
17O, concentrated in the separation by laser of second stage
18O also can be opposite but be somebody's turn to do order.Use separation by laser device 5 present embodiment skeleton diagram as shown in figure 10, this separation by laser device 5 is designed to optionally decompose contain
18Behind the ozone molecule of O, optionally decompose and contain
17The ozone molecule of O.In the present embodiment, also can concentrate
17O and
18O compares with first embodiment, can improve
17The enrichment of O and yield.
The destilling tower that uses specification shown in the table 3 as destilling tower 1, use specification shown in the table 12 the separation by laser device as separation by laser device 5, use the ultra-high purity oxygen of forming shown in the table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in the table 11.Further, the isotopics distribution table of the oxygen in the destilling tower 1 is shown among Figure 11.Concentrating among the P1 as can be known has
17Concentrating among O, the W2 has
18O.
[table 11]
F | W1 | D bot | R | W2 | P1 | ||
Flow [mol/s] | 1.00e-3 | 9.95e-4 | 1.28e-5 | 7.43e-6 | 4.99e-6 | 4.03e-7 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 9.95e-1 7.38e-4 4.07e-3 1.37e-7 1.51e-6 4.16e-6 | 9.98e-1 5.97e-4 1.09e-3 4.88e-8 2.33e-7 3.96e-7 | 5.14e-1 2.01e-2 4.33e-1 6.50e-5 2.72e-3 2.99e-2 | 5.83e-1 1.53e-2 3.46e-1 1.00e-4 4.53e-3 5.12e-2 | 4.96e-1 8.29e-3 4.08e-1 3.46e-5 3.41e-3 8.40e-2 | 5.94e-1 1.67e-1 1.86e-1 1.18e-2 2.62e-2 1.46e-2 |
Isotopic purity [atom%] | 16O 17O 18O | 9.98e-1 3.70e-4 2.04e-3 | 9.99e-1 2.99e-4 5.47e-4 | 7.41e-1 1.15e-2 2.48e-1 | 7.64e-1 1.00e-2 2.26e-1 | 7.04e-1 5.88e-3 2.90e-1 | 7.71e-1 1.08e-1 1.21e-1 |
[table 12]
LIS unit (Type B) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 1.28E-05 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 8.98E-05 | 1.00 | - | - |
(3) | The ozone generator outlet | 8.55E-05 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 1.62E-04 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 7.69E-05 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS phase I charging (O 3,Kr) | 8.55E-05 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 8.71E-05 | 0.06 | 0.06 | 0.88 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2-1 | 4.99E-06 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=LIS second stage charging (O 3,Kr) | 8.22E-05 | - | 0.06 | 0.94 |
(10) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 8.23E-05 | 0.00 | 0.06 | 0.93 |
(11) | O 2Knockout tower cat head=LIS concentrates O 2-2 | 4.03E-07 | 1.00 | - | - |
(12) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 8.19E-05 | - | 0.06 | 0.94 |
(13) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 8.44E-05 | 0.09 | - | 0.91 |
(14) | Kr reclaims outlet (Kr): the Kr internal circulating load | 7.69E-05 | - | - | 1.00 |
(15) | Kr reclaims outlet (O 2): LIS reduces O 2 | 7.43E-06 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 1.48E-03 6.71E-03 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (phase I) | 16O 16O 18O 90% 0.201 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (second stage) | 16O 16O 17O 90% 0.016 |
<the five embodiment 〉
Present embodiment is further to have connected isotope converter 3 on the destilling tower 1 of the 4th embodiment, by present embodiment, can further promote in the destilling tower 1
17O concentrates, and improves
17The enrichment of O and yield.The skeleton diagram of present embodiment as shown in figure 12.
The destilling tower that uses specification shown in the table 3 as destilling tower 1, use specification shown in the table 15 the separation by laser device as separation by laser device 5, use the ultra-high purity oxygen of forming shown in the table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in table 13 and the table 14.Concentrating among the P1 as can be known has
17Concentrating among O, the W2 has
18O.Further, the isotopics distribution table of the oxygen in the destilling tower 1 is shown among Figure 13.
[table 13]
F | W1 | S in | S out | ||
Flow [mol/s] | 1.00e-3 | 9.94e-4 | 1.0e-3 | 1.0e-3 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 9.95e-1 7.38e-4 4.07e-3 1.37e-7 1.51e-6 4.16e-6 | 9.98e-1 5.71e-4 1.01e-3 7.02e-8 2.20e-7 3.35e-7 | 5.50e-1 1.94e-2 3.64e-1 1.70e-4 6.35e-3 5.95e-2 | 5.51e-1 1.94e-2 3.63e-1 1.71e-4 6.40e-3 5.99e-2 |
Isotopic purity [atom%] | 16O 17O 18O | 9.98e-1 3.70e-4 2.04e-3 | 9.99e-1 2.85e-4 5.04e-4 | 7.42e-1 1.31e-2 2.45e-1 | 7.42e-1 1.31e-2 2.45e-1 |
[table 14]
D bot | R | W2 | P1 | ||
Flow [mol/s] | 1.33e-5 | 7.68e-6 | 5.14e-6 | 4.51e-7 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 5.49e-1 1.94e-2 3.65e-1 1.70e-4 6.39e-3 6.00e-2 | 5.84e-1 1.74e-2 3.43e-1 1.30e-4 5.12e-3 5.04e-2 | 4.96e-1 9.44e-3 4.07e-1 4.49e-5 3.87e-3 8.34e-2 | 5.88e-1 1.76e-1 1.82e-1 1.31e-2 2.72e-2 1.41e-2 |
Isotopic purity [atom%] | 16O 17O 18O | 7.41e-1 1.31e-2 2.46e-1 | 7.64e-1 1.14e-2 2.24e-1 | 7.04e-1 6.70e-3 2.89e-1 | 7.67e-1 1.15e-1 1.19e-1 |
[table 15]
LIS unit (Type B) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 1.33E-05 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 9.29E-05 | 1.00 | - | - |
(3) | The ozone generator outlet | 8.85E-05 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 1.68E-04 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 7.96E-05 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS phase I charging (O 3,Kr) | 8.85E-05 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 9.02E-05 | 0.06 | 0.06 | 0.88 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2-1 | 5.14E-06 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=LIS second stage charging (O 3,Kr) | 8.51E-05 | - | 0.06 | 0.94 |
(10) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 8.52E-05 | 0.01 | 0.06 | 0.93 |
(11) | O 2Knockout tower cat head=LIS concentrates O 2-2 | 4.51E-07 | 1.00 | - | - |
(12) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 8.48E-05 | - | 0.06 | 0.94 |
(13) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 8.73E-05 | 0.09 | - | 0.91 |
(14) | Kr reclaims outlet (Kr): the Kr internal circulating load | 7.96E-05 | - | - | 1.00 |
(15) | Kr reclaims outlet (O 2): LIS reduces O 2 | 7.68E-06 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 1.53E-03 6.95E-03 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (phase I) | 16O 16O 18O 90% 0.207 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (second stage) | 16O 16O 17O 90% 0.018 |
<the six embodiment 〉
In the present embodiment, isotope converter 3 and separation by laser device 2 on destilling tower 6, have been connected.Wherein, destilling tower 6 is compared with destilling tower 1 and has only been increased height.In addition, separation by laser device 2 carries out at the tower pars intermedia to the connection of destilling tower 6.On the other hand, with second embodiment similarly, the link position of isotope converter 3 can be at any part of destilling tower 6, but be preferably position or tower bottom near tower bottom.In addition, the position of gas being returned in the destilling tower 6 is not limited especially, can be near the position of gas bleeding or identical position.The skeleton diagram of present embodiment is illustrated among Figure 14.
In the present embodiment, concentrated at the tower bottom of destilling tower 6
18O becomes oxygen P
18On the other hand, inter-level
17O mainly with
16O
17O or
17O
18The form of O is in the concentration maximum of the tower pars intermedia of destilling tower 6.From extracting oxygen D near this tower pars intermedia out
Cut
Then, with oxygen D
CutSupply in the separation by laser device 2, contain by optionally decomposing
17The ozone molecule of O
16O
16O
17O is concentrated
17The oxygen P of O
17, remaining oxygen R turns back in the destilling tower 6.
Present embodiment is characterised in that, by from
17The pars intermedia of the destilling tower 6 of O concentration maximum is extracted oxygen D out
Cut, can separate effectively
17O will
18O is to oxygen P
17Sneak into and suppress to be Min., therefore can prevent block P
18 18The O yield reduces.
And, oxygen D
Cut 17The O enrichment depends on the height of destilling tower 6.For example, P
18 18When the O enrichment was identical, the height of destilling tower 6 was high more, oxygen D
Cut 17The O enrichment is big more.Thus, the height of preferred destilling tower 6 is at least more than the 150m.But, consider from the viewpoint of practicality, be preferably below the 600m.
The destilling tower that uses specification shown in the table 16 as destilling tower 6, use specification shown in the table 19 the separation by laser device as separation by laser device 2, use the ultra-high purity oxygen of forming shown in the table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in table 17 and the table 18.Further, the isotopics distribution table of the oxygen in the destilling tower 6 is shown among Figure 15.And, the oxygen D under this condition
Cut 17O concentration is 0.54atom%.
[table 16]
Destilling tower kind tower diameter packed height filler operating pressure reboiler heat exchange amount | Packed tower 0.120m 200m Φ 5mm Raschig ring (Raschig ring) 20kPa (G) 2.7kW |
[table 17]
F | W1 | S in | S out | ||
Flow [mol/s] | 1.00e-3 | 9.98e-4 | 1.0e-3 | 1.0e-3 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 9.95e-1 7.38e-4 4.07e-3 1.37e-7 1.51e-6 4.16e-6 | 9.98e-1 6.12e-4 1.37e-3 7.61e-8 2.90e-7 2.69e-7 | 2.45e-1 6.20e-3 4.96e-1 3.82e-5 6.16e-3 2.47e-1 | 2.46e-1 6.17e-3 4.94e-1 3.87e-5 6.19e-3 2.48e-1 |
Isotopic purity [atom%] | 16O 17O 18O | 9.98e-1 3.70e-4 2.04e-3 | 9.99e-1 3.06e-4 6.84e-4 | 4.96e-1 6.22e-3 4.98e-1 | 4.96e-1 6.22e-3 4.98e-1 |
[table 18]
D cut | R | P 17 | P 18 | ||
Flow [mol/s] | 3.31e-5 | 3.21e-5 | 1.00e-6 | 1.25e-6 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 5.53e-1 8.13e-3 3.74e-1 2.85e-5 2.66e-3 6.21e-2 | 5.52e-1 5.44e-3 3.77e-1 1.34e-5 1.86e-3 6.43e-2 | 6.30e-1 9.85e-2 2.29e-1 3.85e-3 1.79e-2 2.08e-2 | 6.79e-4 1.08e-4 5.44e-2 4.18e-6 4.02e-3 9.41e-1 |
Isotopic purity [atom%] | 16O 17O 18O | 7.44e-1 5.43e-3 2.50e-1 | 7.43e-1 3.66e-3 2.54e-1 | 7.94e-1 6.21e-2 1.44e-1 | 2.79e-2 2.07e-3 9.70e-1 |
[table 19]
LIS unit (A type) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 3.31E-05 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 2.32E-04 | 1.00 | - | - |
(3) | The ozone generator outlet | 2.20E-04 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 4.19E-04 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 1.98E-04 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS charging (O 3,Kr) | 2.20E-04 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 2.21E-04 | 0.00 | 0.10 | 0.90 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2 | 1.00E-06 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 2.20E-04 | - | 0.10 | 0.90 |
(10) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 2.31E-04 | 0.14 | - | 0.86 |
(11) | Kr reclaims outlet (Kr): the Kr internal circulating load | 1.98E-04 | - | - | 1.00 |
(12) | Kr reclaims outlet (O 2): LIS reduces O 2 | 3.21E-05 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 3.81E-03 1.73E-02 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser | 16O 16O 17O 90% 0.040 |
<the seven embodiment 〉
Present embodiment as shown in figure 16, it is the embodiment that in the 6th embodiment, carries out separation by laser in two stages, separation by laser device 4 (Type B) is identical with the 3rd embodiment, can use in the device of the device of the structure shown in Figure 7 that 2 separation by laser devices 2 (A type) are formed by connecting or structure shown in Figure 8 any one.
For example, in the ozone of phase I decomposes, by optionally decomposing
16O
16O
18O will improve
18The oxygen R1 of O concentration turns back in the destilling tower 6, further in the ozone of second stage decomposes, decomposes by selectivity
16O
16O
17O can further improve
17O concentration and yield.
The destilling tower of specification shown in the use table 16 as destilling tower 6, use specification shown in structure shown in Figure 7, the table 22 the separation by laser device as the ultra-high purity oxygen of forming shown in separation by laser device 4, the use table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in table 20 and the table 21.Further, the isotopics distribution table of the oxygen in the destilling tower 6 is shown among Figure 17.
[table 20]
F | W1 | S in | S out | ||
Flow [mol/s] | 1.00e-3 | 9.98e-4 | 1.0e-3 | 1.0e-3 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 9.95e-1 7.38e-4 4.07e-3 1.37e-7 1.51e-6 4.16e-6 | 9.98e-1 5.95e-4 1.32e-3 6.86e-8 2.50e-7 2.03e-7 | 2.45e-1 5.84e-3 4.96e-1 3.37e-5 5.78e-3 2.47e-1 | 2.46e-1 5.80e-3 4.94e-1 3.41e-5 5.82e-3 2.48e-1 |
Isotopic purity [atom%] | 16O 17O 18O | 9.98e-1 3.70e-4 2.04e-3 | 9.99e-1 2.98e-4 6.61e-4 | 4.96e-1 5.84e-3 4.98e-1 | 4.96e-1 5.84e-3 4.98e-1 |
[table 21]
D cut | R1 | R2 | P 17 | P 18 | ||
Flow [mol/s] | 4.63e-5 | 1.82e-5 | 2.70e-5 | 1.00e-6 | 1.29e-6 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 5.60e-1 7.68e-3 3.69e-1 2.49e-5 2.45e-3 6.01e-2 | 5.02e-1 3.69e-3 4.09e-1 6.78e-6 1.51e-3 8.35e-2 | 5.99e-1 6.72e-3 3.43e-1 1.89e-5 1.92e-3 4.91e-2 | 6.48e-1 1.14e-1 2.00e-1 4.97e-3 1.75e-2 1.54e-2 | 6.85e-4 1.02e-4 5.46e-2 3.69e-6 3.78e-3 9.41e-1 |
Isotopic purity [atom%] | 16O 17O 18O | 7.49e-1 5.09e-3 2.46e-1 | 7.08e-1 2.60e-3 2.89e-1 | 7.74e-1 4.34e-3 2.22e-1 | 8.05e-1 7.05e-2 1.24e-1 | 2.81e-2 1.94e-3 9.70e-1 |
[table 22]
LIS unit (Type B) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 4.63E-05 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 3.24E-04 | 1.00 | - | - |
(3) | The ozone generator outlet | 3.08E-04 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 5.86E-04 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 2.78E-04 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS phase I charging (O 3,Kr) | 3.08E-04 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 3.15E-04 | 0.06 | 0.06 | 0.88 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2-1 | 1.82E-05 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=LIS second stage charging (O 3,Kr) | 2.96E-04 | - | 0.06 | 0.94 |
(10) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 2.97E-04 | 0.00 | 0.06 | 0.94 |
(11) | O 2Knockout tower cat head=LIS concentrates O 2-2 | 1.00E-06 | 1.00 | - | 0.94 |
(12) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 2.96E-04 | - | 0.06 | 0.91 |
(13) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 3.05E-04 | 0.09 | - | 1.00 |
(14) | Kr reclaims outlet (Kr): the Kr internal circulating load | 2.78E-04 | - | - | - |
(15) | Kr reclaims outlet (O 2): LIS reduces O 2 | 2.70E-05 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 5.33E-03 2.42E-02 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (phase I) | 16O 16O 18O 90% 0.733 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (second stage) | 16O 16O 17O 90% 0.040 |
<the eight embodiment 〉
Present embodiment will be compared with the natural abundance ratio
17O is condensed into the oxygen of high concentration as raw material, uses separation by laser device and destilling tower, will
17O is condensed into superelevation enrichment (for example more than the 40atom%).The skeleton diagram of present embodiment is illustrated among Figure 18.
As previously mentioned, in the distillation, maximum boiling point composition and existence are the abundantest
18O concentrates at the tower bottom of destilling tower easily.Therefore, in order effectively will
17O is condensed into ultrahigh concentration, for example, preferably removes from destilling tower as much as possible
18O.Therefore, in the present embodiment, as separating in the oxygen of phase I use separation by laser device 4 from raw material F
18O concentrate oxygen W1 then will as second stage
17O concentrate oxygen D
FeedDeliver in the destilling tower 1.Thus, can suppress in the destilling tower 1
18O concentrates.
In addition, in distillation, if
17O concentration is near ultrahigh concentration (for example more than the 40atom%), then distillation tower height and in the destilling tower that changes relatively
17The O change rate of concentration is little, therefore is difficult to further carry out
17O concentrates.Therefore, in the present embodiment, the tower bottom of destilling tower 1
17When O concentration has just surpassed 40atom%, with oxygen D
BotSupply in the separation by laser device 2, optionally decompose
17O
3, obtain
17O concentrate oxygen P.
Thus, can obtain being condensed into high concentration very effectively
17O.
The destilling tower of specification shown in the use table 3 as destilling tower 1, use specification shown in structure shown in Figure 7, the table 25 the separation by laser device as the separation by laser device of specification shown in separation by laser device 4, the use table 26 as the ultra-high purity oxygen of forming shown in separation by laser device 2, the use table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in table 23 and the table 24.Concentrating among the P as can be known has
17Concentrating among O, the W1 has
18O.Further, the isotopics distribution table of the oxygen in the destilling tower 1 is shown among Figure 19.
[table 23]
F | W1 | W2 | D feed | W3 | ||
Flow [mol/s] | 1.00e-3 | 2.28e-4 | 5.68e-4 | 2.05e-4 | 1.71e-4 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 5.88e-1 1.76e-1 1.82e-1 1.31e-2 2.72e-2 1.41e-2 | 5.15e-1 8.65e-2 3.19e-1 3.63e-3 2.67e-2 4.93e-2 | 6.37e-1 1.56e-1 1.66e-1 9.59e-3 2.03e-2 1.08e-2 | 5.39e-1 3.25e-1 6.59e-2 4.89e-2 1.99e-2 2.01e-3 | 6.91e-1 2.68e-1 2.02e-2 1.73e-2 2.92e-3 1.58e-4 |
Isotopic purity [atom%] | 16O 17O 18O | 7.67e-1 1.15e-1 1.19e-1 | 7.18e-1 6.02e-2 2.22e-1 | 7.98e-1 9.79e-2 1.04e-1 | 7.34e-1 2.21e-1 4.49e-2 | 8.35e-1 1.53e-1 1.17e-2 |
[table 24]
S in | S out | D bot | W4 | P | ||
Flow [mol/s] | 2.05e-4 | 2.05e-4 | 3.39e-5 | 2.45e-5 | 9.44e-6 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 2.75e-1 5.04e-1 6.96e-2 1.29e-1 2.11e-2 1.04e-3 | 3.16e-1 4.40e-1 5.21e-2 1.54e-1 3.63e-2 2.15e-3 | 1.63e-2 2.24e-1 1.91e-1 3.54e-1 1.97e-1 1.81e-2 | 7.06e-2 2.56e-1 1.34e-1 2.33e-1 2.43e-1 6.33e-2 | 1.30e-2 1.77e-1 2.48e-2 6.04e-1 1.69e-1 1.19e-2 |
Isotopic purity [atom%] | 16O 17O 18O | 5.62e-1 3.92e-1 4.63e-2 | 5.62e-1 3.92e-1 4.63e-2 | 2.23e-1 5.65e-1 2.12e-1 | 2.66e-1 4.83e-1 2.52e-1 | 1.14e-1 7.77e-1 1.09e-1 |
[table 25]
LIS unit (Type B) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 1.00E-03 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 7.01E-03 | 1.00 | - | - |
(3) | The ozone generator outlet | 6.67E-03 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 1.27E-02 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 6.01E-03 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS phase I charging (O 3,Kr) | 6.67E-03 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 6.75E-03 | 0.03 | 0.08 | 0.89 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2-1 | 2.28E-04 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=LIS second stage charging (O 3,Kr) | 6.52E-03 | - | 0.08 | 0.92 |
(10) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 6.59E-03 | 0.03 | 0.06 | 0.91 |
(11) | O 2Knockout tower cat head=LIS concentrates O 2-2 | 2.05E-04 | 1.00 | - | - |
(12) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 6.38E-03 | - | 0.06 | 0.94 |
(13) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 6.57E-03 | 0.09 | - | 0.91 |
(14) | Kr reclaims outlet (Kr): the Kr internal circulating load | 6.01E-03 | - | - | 1.00 |
(15) | Kr reclaims outlet (O 2): LIS reduces O 2 | 5.68E-04 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 1.15E-01 5.24E-01 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (phase I) | 16O 16O 18O 90% 9.15 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser (second stage) | 16O 16O 17O 90% 8.22 |
[table 26]
LIS unit (A type) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 3.39E-05 | 1.00 | ||
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 2.38E-04 | 1.00 | ||
(3) | The ozone generator outlet | 2.26E-04 | 0.90 | 0.10 | |
(4) | O 3The knockout tower charging | 4.30E-04 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 2.04E-04 | 1.00 | ||
(6) | O 3At the bottom of the separation Tata=LIS charging (O 3,Kr) | 2.26E-04 | 0.10 | 0.90 | |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 2.29E-04 | 0.04 | 0.07 | 0.89 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2 | 9.44E-06 | 1.00 | ||
(9) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 2.20E-04 | 0.07 | 0.93 | |
(10) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 2.28E-04 | 0.11 | 0.89 | |
(11) | Kr reclaims outlet (Kr): the Kr internal circulating load | 2.04E-04 | 1.00 | ||
(12) | Kr reclaims outlet (O 2): LIS reduces O 2 | 2.45E-05 | 1.00 |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 3.91E-03 1.78E-02 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser | 17O 17O 17O 90% 0.380 |
<the nine embodiment 〉
Present embodiment has further been improved the 8th embodiment as shown in figure 20, has realized
17O concentrates and the raising of yield, is with the difference of the 8th embodiment, uses the separation by laser device 2a of the tower bottom that is connected destilling tower 1 to obtain
17During O concentrate oxygen P, will turn back to from the waste gas R2 of laser separator 2a in the destilling tower 1, further use the separation by laser device 2b of the pars intermedia that is connected destilling tower 1, optionally separate
18O concentrate oxygen W4.
The tower bottom that can suppress thus, destilling tower 1
18O concentrates, so can obtain higher concentration
17O.
The destilling tower that uses specification shown in the table 3 as destilling tower 1, use specification shown in the table 25 the separation by laser device as separation by laser device 4, use specification shown in the table 30 the separation by laser device as separation by laser device 2a, use specification shown in the table 31 the separation by laser device as separation by laser device 2b, use the ultra-high purity oxygen of forming shown in the table 2 as raw material ultra-high purity oxygen F, flow, the isotopics of the oxygen in the device each several part that obtains by computer simulation are illustrated in table 27~table 29.Concentrating among the P as can be known has
17Concentrating among O, the W1 has
18O.Further, the isotopics distribution table of the oxygen in the destilling tower 1 is shown among Figure 21.
[table 27]
F | W1 | W2 | D feed | W3 | ||
Flow [mol/s] | 1.00e-3 | 2.28e-4 | 5.68e-4 | 2.05e-4 | 5.39e-5 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 5.88e-1 1.76e-1 1.82e-1 1.31e-2 2.72e-2 1.41e-2 | 5.15e-1 8.65e-2 3.19e-1 3.63e-3 2.67e-2 4.93e-2 | 6.37e-1 1.56e-1 1.66e-1 9.59e-3 2.03e-2 1.08e-2 | 5.39e-1 3.25e-1 6.59e-2 4.89e-2 1.99e-2 2.01e-3 | 8.00e-1 1.85e-1 4.41e-3 9.96e-3 4.74e-4 1.60e-5 |
Isotopic purity [atom%] | 16O 17O 18O | 7.67e-1 1.15e-1 1.19e-1 | 7.18e-1 6.02e-2 2.22e-1 | 7.98e-1 9.79e-2 1.04e-1 | 7.34e-1 2.21e-1 4.49e-2 | 8.95e-1 1.03e-1 2.46e-3 |
[table 28]
D cut | R1 | W4 | S in | ||
Flow [mol/s] | 8.21e-3 | 8.07e-3 | 1.44e-4 | 2.05e-4 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 5.40e-1 3.85e-1 4.65e-3 6.81e-2 1.55e-3 5.06e-5 | 5.41e-1 3.86e-1 3.14e-3 6.87e-2 1.12e-3 4.56e-6 | 4.98e-1 3.31e-1 8.47e-2 5.49e-2 2.81e-2 3.60e-3 | 2.52e-1 5.00e-1 1.40e-2 2.24e-1 9.72e-3 1.67e-4 |
Isotopic purity [atom%] | 16O 17O 18O | 7.35e-1 2.62e-1 3.15e-3 | 7.36e-1 2.62e-1 2.14e-3 | 7.06e-1 2.34e-1 6.00e-2 | 5.09e-1 4.79e-1 1.20e-2 |
[table 29]
S out | D bot | R2 | P | ||
Flow [mol/s] | 2.05e-4 | 1.28e-5 | 5.96e-6 | 6.87e-6 | |
Form [mol%] | 16O 2 16O 17O 16O 18O 17O 2 17O 18O 18O 2 | 2.59e-1 4.88e-1 1.22e-2 2.29e-1 1.15e-2 1.44e-4 | 1.42e-2 1.91e-1 3.96e-2 5.73e-1 1.64e-1 1.88e-2 | 4.15e-2 2.47e-1 7.71e-2 3.69e-1 2.30e-1 3.58e-2 | 4.25e-3 1.14e-1 7.92e-3 7.64e-1 1.06e-1 3.69e-3 |
Isotopic purity [atom%] | 16O 17O 18O | 5.09e-1 4.79e-1 1.20e-2 | 1.30e-1 7.50e-1 1.20e-1 | 2.04e-1 6.07e-1 1.89e-1 | 6.52e-2 8.74e-1 6.08e-2 |
[table 30]
LIS unit (A type) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 8.21E-03 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 5.75E-02 | 1.00 | - | - |
(3) | The ozone generator outlet | 5.48E-02 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 1.04E-01 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 4.93E-02 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS charging (O 3,Kr) | 5.48E-02 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 5.48E-02 | 0.00 | 0.10 | 0.90 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2 | 1.44E-04 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 5.47E-02 | - | 0.10 | 0.90 |
(10) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 5.74E-02 | 0.14 | - | 0.86 |
(11) | Kr reclaims outlet (Kr): the Kr internal circulating load | 4.93E-02 | - | - | 1.00 |
(12) | Kr reclaims outlet (O 2): LIS reduces O 2 | 8.07E-03 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 9.46E-01 4.30E+00 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser | 16O 16O 18O 90% 5.79 |
[table 31]
LIS unit (A type) | Flow | Molar fraction | |||
[mol/s] | O 2 | O 3 | Kr | ||
(1) | LIS unit feed (O 2) | 1.28E-05 | 1.00 | - | - |
(2) | Ozone generator inlet: ozone generator O 2Treating capacity | 8.98E-05 | 1.00 | - | - |
(3) | The ozone generator outlet | 8.55E-05 | 0.90 | 0.10 | - |
(4) | O 3The knockout tower charging | 1.63E-04 | 0.47 | 0.05 | 0.47 |
(5) | O 3Knockout tower cat head=O 2Waste gas | 7.70E-05 | 1.00 | - | - |
(6) | O 3At the bottom of the separation Tata=LIS charging (O 3,Kr) | 8.55E-05 | - | 0.10 | 0.90 |
(7) | LIS outlet=O 2Knockout tower charging (O 2,O 3,Kr) | 8.78E-05 | 0.08 | 0.05 | 0.88 |
(8) | O 2Knockout tower cat head=LIS concentrates O 2 | 6.87E-06 | 1.00 | - | - |
(9) | O 2At the bottom of the separation Tata=ozonolysis equipment inlet (O 3,Kr) | 8.10E-05 | - | 0.05 | 0.95 |
(10) | Ozonolysis equipment outlet=Kr reclaims inlet (O 2,Kr) | 8.29E-05 | 0.07 | - | 0.93 |
(11) | Kr reclaims outlet (Kr): the Kr internal circulating load | 7.70E-05 | - | - | 1.00 |
(12) | Kr reclaims outlet (O 2): LIS reduces O 2 | 5.96E-06 | 1.00 | - | - |
Ozone generator unit consumption [gO 3/ kWh] ozone generator O 3Generation [kgO 3/ h] ozone generator power consumption [kW] | 220 1.48E-03 6.72E-03 |
The resolution ratio laser output power [W] of the above-mentioned object of object of separation by laser | 17O 17O 17O 90% 0.275 |
Embodiment
(embodiment 1)
Under the condition of first embodiment, concentrate
17O and
18The simulation of O, the result obtains containing 9.1atom% as can be known
17The oxygen of O and contain 25.2atom%
18The oxygen of O.
17The yield of O is 5.8%,
18The yield of O is 69.8%.
For example, among the embodiment 1
17The numerical value of the yield use table 5 of O is tried to achieve by following formula.
Yield [%]=
(flow
P* isotopic purity
17O
P)/(flow
F* isotopic purity
17O
F) * 100
18The yield of O also uses identical calculating formula to try to achieve.
(embodiment 2)
Under the condition of second embodiment, concentrate
17O and
18The simulation of O, the result obtains containing 10.3atom% as can be known
17The oxygen of O and contain 25.2atom%
18The oxygen of O.
17The yield of O is 7.8%,
18The yield of O is 73.1%, compares with embodiment 1 to some extent and rises.
(embodiment 3)
Under the condition of the 3rd embodiment, concentrate
17O and
18The simulation of O, the result obtains containing 9.7atom% as can be known
17The oxygen of O.
17The yield of O is 14.1%, compares with embodiment 1 to some extent and rises.
18The yield of O is 69.8%, and is identical with embodiment 1, still
18The isotopic purity of O is 29.2atom%, obtains comparing with embodiment 1 containing high-purity
18The oxygen of O.
(embodiment 4)
Under the condition of the 4th embodiment, concentrate
17O and
18The simulation of O, the result obtains containing 10.8atom% as can be known
17The oxygen of O and contain 29.0atom%
18The oxygen of O.
17The yield of O is 11.8%, compares with embodiment 1 to increase.
18The yield of O is 70.9%.
(embodiment 5)
Under the condition of the 5th embodiment, concentrate
17O and
18The simulation of O, the result obtains containing 11.5atom% as can be known
17The oxygen of O and contain 28.9atom%
18The oxygen of O.In addition,
17The yield of O is 14.0%,
18The yield of O is 72.8%.
(embodiment 6)
Under the condition of the 8th embodiment, concentrate
17O and
18The simulation of O, the result obtains containing 77.7atom% as can be known
17The oxygen of O and contain 22.2atom%
18The oxygen of O.
(embodiment 7)
Under the condition of the 9th embodiment, concentrate
17O and
18The simulation of O, the result obtains containing 87.4atom% as can be known
17The oxygen of O and contain 22.2atom%
18The oxygen of O.
By the method for concentration of oxygen isotope of the present invention, confirmed the stable isotope of oxygen that can abundance ratio is very little
17O and
18O is condensed into high concentration effectively.In addition, confirmed when concentrating, compared with prior art finished with the short starting time, therefore can be with low-cost and under commercial scale, obtain high concentration
17O and
18O.
Further, use method for concentration by oxygen isotope of the present invention to obtain
17O or
18The O concentrate oxygen can and obtain having concentrated under commercial scale with low cost
17O or
18The heavy oxygen water of O.
Utilizability on the industry
By the present invention, can under commercial scale, provide at an easy rate17O or18The O concentrate oxygen, so the present invention is inciting somebody to action17O or18The O labeled compound is as being useful in the fields such as the chemistry of tracer or medical science.
Claims (11)
1, a kind of method for concentration of oxygen isotope wherein, comprises the distillation process of the isotopic oxygen of concentrate oxygen and ozone is carried out photodissociation and the concentrate oxygen isotope
17The operation of O.
2, the method for concentration of oxygen isotope according to claim 1 wherein, comprises the operation of carrying out the isotope conversion.
3, the method for concentration of oxygen isotope according to claim 1 wherein, comprises ozone is carried out photodissociation and reduces oxygen isotope
18The operation of O.
4, the method for concentration of oxygen isotope according to claim 3 wherein, comprises the operation of carrying out the isotope conversion.
5, the method for concentration of oxygen isotope according to claim 1, wherein, to the distillation process of the isotopic oxygen of concentrate oxygen, ozone is carried out photodissociation and the concentrate oxygen isotope
17At least a operation in the operation of O is carried out more than twice.
6, the method for concentration of oxygen isotope according to claim 2, wherein, to the distillation process of the isotopic oxygen of concentrate oxygen, ozone is carried out photodissociation and the concentrate oxygen isotope
17The operation of O and at least a operation of carrying out in the operation of isotope conversion are carried out more than twice.
7, the method for concentration of oxygen isotope according to claim 3, wherein, to the distillation process of the isotopic oxygen of concentrate oxygen, ozone is carried out photodissociation and the concentrate oxygen isotope
17The operation of O and ozone carried out photodissociation and reduce oxygen isotope
18At least a operation in the operation of O is carried out more than twice.
8, the method for concentration of oxygen isotope according to claim 4, wherein, to the distillation process of the isotopic oxygen of concentrate oxygen, ozone is carried out photodissociation and the concentrate oxygen isotope
17The operation of O, ozone is carried out photodissociation and reduces oxygen isotope
18The operation of O and at least a operation of carrying out in the operation of isotope conversion are carried out more than twice.
9, the method for concentration of oxygen isotope according to claim 3 wherein, is reducing oxygen isotope
18Carry out the concentrate oxygen isotope after the operation of O
17The operation of O.
10, the method for concentration of oxygen isotope according to claim 3 wherein, is carrying out the concentrate oxygen isotope
17Reduce oxygen isotope after the operation of O
18The operation of O.
11, a kind of manufacture method of heavy oxygen water wherein, obtains to the method for concentration by any described oxygen isotope in the claim 1~9
17The O concentrate oxygen and/or
18The O concentrate oxygen adds hydrogen, obtains oxygen isotope
17O and/or oxygen isotope
18O is condensed into the water of the above concentration of 1atom%.
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JP5415105B2 (en) * | 2009-02-26 | 2014-02-12 | 大陽日酸株式会社 | Oxygen isotope enrichment apparatus and enrichment method |
JP5813613B2 (en) | 2012-10-18 | 2015-11-17 | 大陽日酸株式会社 | Oxygen isotope enrichment method |
JP6172684B2 (en) * | 2015-01-20 | 2017-08-02 | 大陽日酸株式会社 | Oxygen isotope enrichment method |
US10751431B2 (en) * | 2016-06-23 | 2020-08-25 | National Guard Health Affairs | Positron emission capsule for image-guided proton therapy |
JP6606522B2 (en) * | 2017-03-28 | 2019-11-13 | 大陽日酸株式会社 | Carbon monoxide stable isotope enrichment apparatus and carbon monoxide stable isotope enrichment method |
KR102205241B1 (en) | 2018-11-27 | 2021-01-20 | 한국원자력연구원 | Method for the Separation of Carbon Isotope and method for concentrating Carbon isotope |
JP7161391B2 (en) * | 2018-12-07 | 2022-10-26 | 大陽日酸株式会社 | Oxygen-containing compound production method and its production apparatus |
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US6461583B1 (en) * | 1998-11-09 | 2002-10-08 | Nippon Sanso Corporation | Method for enrichment of heavy component of oxygen isotopes |
WO2004078325A1 (en) * | 2003-03-04 | 2004-09-16 | Taiyo Nippon Sanso Corporation | Method for concentrating oxygen isotope |
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US4029559A (en) | 1976-06-17 | 1977-06-14 | The United States Of America As Represented By The United States Energy Research And Development Administration | Ion laser isotope enrichment by photo-predissociation of formaldehyde |
US4029558A (en) | 1976-10-22 | 1977-06-14 | The United States Of America As Represented By The United States Energy Research And Development Administration | Isotope enrichment by frequency-tripled temperature tuned neodymium laser photolysis of formaldehyde |
JP4495279B2 (en) * | 1999-10-12 | 2010-06-30 | 大陽日酸株式会社 | Distillation apparatus, oxygen isotope weight component concentration method, and heavy oxygen water production method |
JP4364529B2 (en) | 2003-03-04 | 2009-11-18 | 大陽日酸株式会社 | Oxygen isotope enrichment method and apparatus |
JP4406228B2 (en) | 2003-07-24 | 2010-01-27 | 大陽日酸株式会社 | Oxygen isotope enrichment method and apparatus |
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US6461583B1 (en) * | 1998-11-09 | 2002-10-08 | Nippon Sanso Corporation | Method for enrichment of heavy component of oxygen isotopes |
WO2004078325A1 (en) * | 2003-03-04 | 2004-09-16 | Taiyo Nippon Sanso Corporation | Method for concentrating oxygen isotope |
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CN111195482A (en) * | 2018-11-16 | 2020-05-26 | 韩国原子力研究院 | Method for separating O-17 isotope from water and method for concentrating O-17 isotope |
US11286161B2 (en) | 2018-11-16 | 2022-03-29 | Korea Atomic Energy Research Institute | Process for isolating 170 isotope from water and process for concentrating 170 isotope using the same |
CN111195482B (en) * | 2018-11-16 | 2022-04-01 | 韩国原子力研究院 | Method for separating O-17 isotope from water and method for concentrating O-17 isotope |
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US8337802B2 (en) | 2012-12-25 |
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CN101242888B (en) | 2012-09-05 |
WO2007020934A1 (en) | 2007-02-22 |
EP1923126A1 (en) | 2008-05-21 |
JPWO2007020934A1 (en) | 2009-02-26 |
US20090035212A1 (en) | 2009-02-05 |
EP1923126B1 (en) | 2019-06-19 |
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